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Title: Enhanced Iron Solubility at Low pH in Global Aerosols

The composition and oxidation state of aerosol iron were examined using synchrotron-based iron near-edge X-ray absorption spectroscopy. By combining synchrotron-based techniques with water leachate analysis, impacts of oxidation state and mineralogy on aerosol iron solubility were assessed for samples taken from multiple locations in the Southern and the Atlantic Oceans; and also from Noida (India), Bermuda, and the Eastern Mediterranean (Crete). These sampling locations capture iron-containing aerosols from different source regions with varying marine, mineral dust, and anthropogenic influences. Across all locations, pH had the dominating influence on aerosol iron solubility. When aerosol samples were approximately neutral pH, iron solubility was on average 3.4%; when samples were below pH 4, the iron solubility increased to 35%. This observed aerosol iron solubility profile is consistent with thermodynamic predictions for the solubility of Fe(III) oxides, the major iron containing phase in the aerosol samples. Source regions and transport paths were also important factors affecting iron solubility, as samples originating from or passing over populated regions tended to contain more soluble iron. Although the acidity appears to affect aerosol iron solubility globally, a direct relationship for all samples is further confounded by factors such as anthropogenic influence, aerosol buffer capacity, mineralogy and physicalmore » processes.« less
Authors:
 [1] ;  [2] ;  [1] ;  [3] ; ORCiD logo [4] ;  [4] ; ORCiD logo [5] ;  [6] ;  [7] ; ORCiD logo [8] ;  [9] ;  [10] ;  [1]
  1. Georgia Inst. of Technology, Atlanta, GA (United States). School of Earth and Atmospheric Sciences
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Environmental Science Division
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  4. Florida State Univ., Tallahassee, FL (United States). Earth, Ocean and Atmospheric Science
  5. Florida State Univ., Tallahassee, FL (United States). National High Magnetic Field Lab. (MagLab)
  6. Georgia Inst. of Technology, Atlanta, GA (United States). School of Earth and Atmospheric Sciences and School of Chemical and Biomolecular Engineering; Foundation for Research & Technology-Hellas, Crete (Greece). Inst. of Chemical Engineering Sciences; National Observatory of Athens (NOA), Penteli (Greece). Inst. for Environmental Research and Sustainable Development (IERSD)
  7. National Observatory of Athens (NOA), Penteli (Greece). Inst. for Environmental Research and Sustainable Development (IERSD); Univ. of Crete, Heraklion (Greece). Dept. of Chemistry
  8. Univ. of Crete, Heraklion (Greece). Dept. of Chemistry
  9. Rutgers Univ., Newark, NJ (United States). Dept. of Earth and Environmental Sciences
  10. Amity Univ., Noida (India). Amity Inst. of Environmental Sciences; Adigrat Univ. (Ethiopia). Dept. of Environmental Science
Publication Date:
Grant/Contract Number:
AC02-06CH11357; OCE 1357375; OCE 1658181; OCE-0929919; OCE-1034764; OCE-1658311; OPP-0944589; PLR-1341494; DMR-1157490
Type:
Accepted Manuscript
Journal Name:
Atmosphere (Basel)
Additional Journal Information:
Journal Name: Atmosphere (Basel); Journal Volume: 9; Journal Issue: 5; Journal ID: ISSN 2073-4433
Publisher:
MDPI
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF); European Union (EU)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; aerosol chemistry; aerosol iron; aerosol pH; iron solubility; synchrotron
OSTI Identifier:
1462692

Ingall, Ellery, Feng, Yan, Longo, Amelia, Lai, Barry, Shelley, Rachel, Landing, William, Morton, Peter, Nenes, Athanasios, Mihalopoulos, Nikolaos, Violaki, Kalliopi, Gao, Yuan, Sahai, Shivraj, and Castorina, Erin. Enhanced Iron Solubility at Low pH in Global Aerosols. United States: N. p., Web. doi:10.3390/atmos9050201.
Ingall, Ellery, Feng, Yan, Longo, Amelia, Lai, Barry, Shelley, Rachel, Landing, William, Morton, Peter, Nenes, Athanasios, Mihalopoulos, Nikolaos, Violaki, Kalliopi, Gao, Yuan, Sahai, Shivraj, & Castorina, Erin. Enhanced Iron Solubility at Low pH in Global Aerosols. United States. doi:10.3390/atmos9050201.
Ingall, Ellery, Feng, Yan, Longo, Amelia, Lai, Barry, Shelley, Rachel, Landing, William, Morton, Peter, Nenes, Athanasios, Mihalopoulos, Nikolaos, Violaki, Kalliopi, Gao, Yuan, Sahai, Shivraj, and Castorina, Erin. 2018. "Enhanced Iron Solubility at Low pH in Global Aerosols". United States. doi:10.3390/atmos9050201. https://www.osti.gov/servlets/purl/1462692.
@article{osti_1462692,
title = {Enhanced Iron Solubility at Low pH in Global Aerosols},
author = {Ingall, Ellery and Feng, Yan and Longo, Amelia and Lai, Barry and Shelley, Rachel and Landing, William and Morton, Peter and Nenes, Athanasios and Mihalopoulos, Nikolaos and Violaki, Kalliopi and Gao, Yuan and Sahai, Shivraj and Castorina, Erin},
abstractNote = {The composition and oxidation state of aerosol iron were examined using synchrotron-based iron near-edge X-ray absorption spectroscopy. By combining synchrotron-based techniques with water leachate analysis, impacts of oxidation state and mineralogy on aerosol iron solubility were assessed for samples taken from multiple locations in the Southern and the Atlantic Oceans; and also from Noida (India), Bermuda, and the Eastern Mediterranean (Crete). These sampling locations capture iron-containing aerosols from different source regions with varying marine, mineral dust, and anthropogenic influences. Across all locations, pH had the dominating influence on aerosol iron solubility. When aerosol samples were approximately neutral pH, iron solubility was on average 3.4%; when samples were below pH 4, the iron solubility increased to 35%. This observed aerosol iron solubility profile is consistent with thermodynamic predictions for the solubility of Fe(III) oxides, the major iron containing phase in the aerosol samples. Source regions and transport paths were also important factors affecting iron solubility, as samples originating from or passing over populated regions tended to contain more soluble iron. Although the acidity appears to affect aerosol iron solubility globally, a direct relationship for all samples is further confounded by factors such as anthropogenic influence, aerosol buffer capacity, mineralogy and physical processes.},
doi = {10.3390/atmos9050201},
journal = {Atmosphere (Basel)},
number = 5,
volume = 9,
place = {United States},
year = {2018},
month = {5}
}

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